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Paleoclimatic indication of X-ray fluorescence core-scanned Rb/Sr ratios: A

case study in the Zoige Basin in the eastern Tibetan Plateau

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DOI: 10.1007/s11430-020-9667-7

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 SCIENCE CHINA
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............................

Paleoclimatic indication of X-ray fluorescence core-scanned Rb/Sr

ratios: A case study in the Zoige Basin in the eastern Tibetan
Plateau
1,2 1,2 1* 1,2 1
Hanfei YANG , Yan ZHAO , Qiaoyu CUI , Weihe REN & Quan LI
1
Key Laboratory of Land Surface Pattern and Simulation, Institute of Geographic Sciences and Natural Resources Research, Chinese Academy
of Sciences, Beijing 100101, China;
2
University of Chinese Academy of Sciences, Beijing 100049, China

Received January 21, 2020; revised June 27, 2020; accepted July 30, 2020; published online October 16, 2020

Abstract The X-ray fluorescence (XRF) core-scanned Rb/Sr ratios of lake sediments have been widely used as a proxy for
chemical weathering intensity and past climate change. However, some factors could affect Rb/Sr ratios, causing mis-
interpretation and limiting its application. In this study, we present a high-resolution XRF core-scanned Rb/Sr record of core
ZB13-C1 from the Zoige Basin in the eastern Tibetan Plateau. To validate its application, we correlated this record with the
chemical index of alteration (CIA) and other paleoclimatic proxies. Our results showed that (1) the core-scanned Rb/Sr ratios and
CIA were reliable proxies of chemical weathering intensity in fine-grained sedimentary sequences; (2) the low values of core-
scanned Rb/Sr ratios and CIA were significantly correlated with high total organic carbon content, arboreal pollen content,
carbonate content, and C/N ratios, confirming its reliability as a proxy for the Asian summer monsoon intensity; (3) the core-
scanned Rb/Sr ratios at core depths of 25–0.3 and 56–47 m were unable to reliably reflect chemical weathering intensity due to
both the grain-size effect and the low test accuracy. Our study highlights the need for mutual verification of multiple indicators
before accurately applying Rb/Sr as a paleoclimatic proxy in other similar study areas.
Keywords Rb/Sr ratios, XRF core scanning, Lake sediment, Tibetan Plateau, Paleoclimatic indication

Citation: Yang H, Zhao Y, Cui Q, Ren W, Li Q. 2020. Paleoclimatic indication of X-ray fluorescence core-scanned Rb/Sr ratios: A case study in the Zoige Basin
in the eastern Tibetan Plateau. Science China Earth Sciences, 63, https://doi.org/10.1007/s11430-020-9667-7

1. Introduction 2018); this is based on the assumption that chemical

The X-Ray fluorescence (XRF) core scanning has been in-
creasingly applied since the late 1980s due to its rapid ac-
quirement of high-resolution geochemistry data (Jansen et
al., 1998). Many proxies based on XRF elemental ratios have
been used as indicators of past climatic and environmental
changes across a wide range of timescales (Croudace and
Rothwell, 2015). In particular, Rb/Sr ratios have been widely
applied to reflect chemical weathering intensity and climate
change on geological timescales (Wu et al., 2006; Fritz et al.,
* Corresponding author (email: qiaoyu.cui@igsnrr.ac.cn)
weathering intensity is a function of temperature and rainfall/
moisture (Jin and Zhang, 2002). Previous studies in the early
1960s inferred a positive correlation between Rb/Sr ratios in
weathered clastic rocks and chemical weathering intensity
(Bottino and Fullagar, 1968; Dasch, 1969). Subsequently, the
87 86
Rb/Sr ratios (or Rb/ Sr) of loess-paleosol archives were
used to reconstruct their provenance, weathering process,
and pedogenesis (Gallet et al., 1996; Sun, 2002) as well as
the intensity of the East Asian summer monsoon (Chen et al.,
1999a, 1999b; Chen et al., 2003). Rb/Sr ratios of lake sedi-
ments have been increasingly applied over the past few
decades. For example, Jin et al. (2001, 2006) used Rb/Sr

© Science China Press and Springer-Verlag GmbH Germany, part of Springer Nature 2020 earth.scichina.com link.springer.com
2 Yang H, et al.
ratios to reconstruct Holocene chemical weathering varia-
bility in the Daihai Lake catchment. More recently, Rb/Sr
ratios have been considered an index for the evolution of the
Asian summer monsoon (An et al., 2011; Si et al., 2014;
Zhao et al., 2020) and the Westerlies (Chang et al., 2013).
A variety of factors are known to influence Rb/Sr ratios,
including climatic factors, vegetation cover, the chemical/
physical properties of the source rock, and enhanced human
activity over the past thousands of years; this can lead to
misinterpretations and significantly limit its application. For
example, Rb/Sr variability may result from the alterations of
sediment source under weak weathering conditions as op-
posed to changes in weathering intensity (Ren et al., 2019).
Meanwhile, Rb/Sr ratios have also been used as an indicator
of sediment supply from terrestrial unweathered clastic rocks
(Kalugin et al., 2005, 2007). Moreover, the effect of grain-
size sorting during sedimentation could enrich Rb in the clay
fraction and Sr in the silt and sand fractions (Shen H Y et al.,
2006; Zeng et al., 2011). To minimise the influence of grain
size, some studies have suggested the use of only fine sedi-
ments to measure weathering intensity (Xiong et al., 2010;
Bao et al., 2019). Furthermore, Sr migration in loess deposits
is primarily controlled by carbonate minerals by displacing
Ca in carbonates (Wedepohl, 1978). Secondary carbonates
formed during the post-pedogenetic process would likely
mask the influence of silicate weathering and leaching in-
tensity in paleosols. To avoid the bias from secondary car-
bonates, studies have suggested the use of carbonate-free
parent materials for the measurement of Sr in loess-paleosol
deposits (Buggle et al., 2011). Understanding the limitations
of Rb/Sr ratios and its controlling factors are fundamental for
its application and interpretation.
The climate of the eastern Tibetan Plateau (TP) is sensitive
to global climate change. Multiple proxies have been used to
reconstruct the Holocene paleoclimatology of the eastern TP,
including grain size, magnetic susceptibility, stable isotopes,
and pollen assemblages preserved in loess and peat deposits
(Zhao et al., 2014; Wen et al., 2017; Wang et al., 2018; Li and
Zhao, 2019). Sedimentary proxies in lake sediments have
also been used for paleoclimate reconstructions in the Qai-
dam Basin in the northeastern TP (Jian et al., 2013; Ren et
al., 2019). A large number of paleoclimatic studies have
investigated the peat profiles of the Zoige Basin due to its
highly developed peat depositional environment. Studies on
a number of peat sections from the Hongyuan area since the
1980s have developed precise chronological frameworks,
paleoenvironmental histories, and paleoclimatic evolutions
since the late glacial epoch (Wang et al., 1993, 1996; Sun et
al., 2001; Zhou et al., 2001; Wang et al., 2006; Yu et al.,
2006). Two long lacustrine sedimentary cores—RH and RM
—were retrieved in 1992 and 1993 from the centre of the
Zoige Basin, covering 0.9 million years of climate change on
the eastern TP (Wang and Xue, 1997). However, most of
Sci China Earth Sci
these studies focused on palynological, isotopic, lithological,
and magnetic susceptibility analyses (Liu et al., 1994; Wang
et al., 1995a, 1995b; Chen et al., 1999; Hu et al., 1999; Wu et
al., 2000; Shen et al., 2005). To date, there are still few
palaeoclimatic reconstructions in the Zoige Basin based on
geochemical proxies, including Rb/Sr ratios.
In this study, we present records of XRF core-scanned
(XRFCS) Rb/Sr, chemical index of alteration (CIA), total
organic carbon (TOC) content, C/N ratios, and traditional-
XRF-derived (XRFT) Rb/Sr from core ZB13-C1 in the Zoige
Basin. The study aims to (1) compare XRFCS Rb/Sr ratios
with CIA to verify its application as a paleoclimatic proxy;
(2) compare XRFCS Rb/Sr ratios with multiple proxies (TOC
content, C/N ratio, arboreal pollen (AP) content, and car-
bonate content) to validate its application as a proxy for the
Asian summer monsoon intensity; and (3) evaluate the in-
fluence of grain size on XRFCS Rb/Sr ratios through com-
parisons with XRFT Rb/Sr ratios, CIA, and grain-size data.
We assess the accuracy of XRFCS Rb/Sr ratios as an index for
chemical weathering intensity in the lake catchment. Our
results significantly contribute towards the interpretation and
reconstruction of paleoclimatic changes on the eastern TP.
2. Study area
The Zoige Basin is located on the eastern TP (Figure 1a) and
2
covers an area and altitude range of ca. 19,400 km and
3400–3600 m a.s.l. (meter above sea level), respectively. The
mountains surrounding the basin reach elevations of 4000–
5000 m a.s.l. The ancient lake in the Zoige Basin was formed
before ca. 40 ka BP (Wang et al., 1995b; Xue et al., 1998),
and the lacustrine sedimentary sequence in the central basin
has a thickness of >300 m (Xue et al., 1998). The major
rivers in the basin include the Yellow River and its tribu-
taries, such as the White River, Black River, and Jiaqu River.
The climate in the Zoige Basin is mainly influenced by the
Asian monsoon and the Westerlies (Ye and Gao, 1979; Ding,
1992). According to the 1987–2016 observational data from
the Zoige meteorological station, the mean annual tempera-
ture in the Zoige Basin is 1.9°C (the minimum and maximum
monthly temperature is −9.0°C in January and 11.5°C in
July, respectively), and the mean annual precipitation is
654.3 mm (mainly from May to September) (Figure 1b). The
vegetation in the Zoige Basin is dominated by sedge marshes
consisting of Carex muliensis and Kobresia humilis. The
terraces and mountain slopes at 3400–3800 m a.s.l. are
covered by subalpine meadows composed of K. setchwa-
nensis, Clinelymus nutans, Poa partensis, and other plants
belonging to Asteraceae, Ranunculaceae, and Fabaceae. The
high-altitude slopes up to 4000 m a.s.l. are occupied by al-
pine coniferous forest, including Picea asperata, P. wilsonii,
P. purpurea, Abies faxoniana, Pinus densata, Betula platy-
 Yang H, et al.
Figure 1 Location and climate of the Zoige Basin on the eastern Tibetan Plateau. (a) Locations of core ZB13-C1 and the Zoige meteorological station. (b)
Meteorological data from the Zoige station (33°35′N, 102°58′E, 3441.4 m a.s.l.) showing monthly mean temperature and precipitation during 1987–2016.
Meteorological data were from the National Meteorological Information Center (source: http://data.cma.cn).
phylla, and Quercus liaotunggensis (Shen et al., 2005).
3. Materials and methods
3.1 Core description
Core ZB13-C1 (33°54.72′N, 102°41.39′E, 3458 m a.s.l.) was
drilled near the sedimentary centre of the Zoige Basin in
2013 (Figure 1a). The core penetrated ca. 110 m of mostly
lacustrine sediments (0.33–106.01 m) at a total core acqui-
sition rate of 91%. The recovered core was split into two
parts: one half was used for multi-proxy analysis and the
other half for XRF core scanning.
The lithology of the core mainly consists of clay and silty
clay, which accounts for ~26% and 40% of the entire core,
respectively. Silt, clayey silt, and fine sand only contribute
~6%, 13%, and 7% of the entire core, respectively. The se-
diments of the top 30 m are dominated by the coarse fraction
(grain size >63 μm) composed of blue-grey silt and fine sand
intercalated with organic-rich thin layers. Four distinct or-
ganic layers occur at depths of 84.83–82.88, 68.22–67.58,
64.19–63.23, and 46.05–44.93 m. Several calcareous con-
cretions occur at depths of 91.70, 70.50–69.90, 12.50, and
7.45 m (Figure 2).
3.2 XRF core scanning
XRF core scanning was conducted using the Avaatech XRF
Core Scanner (Richter et al., 2006) at the Key Laboratory of
Western China’s Environmental Systems (Ministry of Edu-
Sci China Earth Sci 3
cation of China), Lanzhou University. Al, Si, K, Ca, Ti, and
Fe measurements were preformed every 1 cm at an exposure
time of 15 s, a voltage of 10 kV, and a current of 1 mA; Rb,
Sr, and Zr measurements were performed at an exposure time
of 25 s, a voltage of 30 kV, and a current of 2 mA. To
minimise the influence of measurement geometry (i.e. irre-
gularities in the core surface) and to prevent the core samples
from contaminating the XRF probe, the core surface was
smoothed and covered by a 4 μm thick Ultralene film before
scanning. The element data detected by the Avaatech Scan-
ner are presented as counts per second (cps). The data are
semi-quantitative, reflecting the relative changes of chemical
composition rather than the absolute concentration. Element
values lower than 500 cps were excluded due to their low
reliability and accounted for 0.34% of the total number of
scanning points.
A principal component analysis (PCA) was conducted on
the XRF-scanned elements—Si, Al, Ti, K, Rb, Zr, Fe, Ca,
and Sr—to objectively extract the dominant information
(variance) preserved in the dataset. To overcome the closed-
sum effect in compositional data that leads to spurious cor-
relations between the geochemical elements (Rollinson,
1993), all the XRF data were log-transformed before PCA by
calculating the centred log ratios (Aitchison, 1982).
3.3 Traditional XRF analysis
A total of 512 subsamples at 2-cm thickness were collected
from core ZB13-C1 at ~20-cm intervals for traditional XRF
analysis. Several oxides were obtained to calculate the car-
4 Yang H, et al.
Figure 2 Lithological column of core ZB13-C1 from the Zoige Basin on the eastern Tibetan Plateau. Blank sections indicate gaps in the record as a result of
drilling.
*
bonate-free CIA (CIA=[Al2O3/(Al2O3+CaO +Na2O+K2O)]×
*
100 (in molar proportions), where CaO is the molar content
of CaO in silicate minerals). The dried samples were ground
into 200 mesh powder using an agate mortar, and 6 g of each
−1
powdered sample was acid-hydrolysed in 1 mol L acetic
acid for >10 h at room temperature to remove the carbonate
fraction (Jackson, 1956). The acid residues were rinsed 3
times with distilled water and then dried. Approximately
0.7±0.0003 g of dried sample powder was calcined in a
muffle furnace for 1 h at 1000°C. The samples were then
fully mixed with 7±0.0003 g of dry lithium tetraborate (Li2
B4O7) and fused to a glass sheet in platinum crucibles at
1000°C for traditional XRF analysis. The abundances of
major and trace elements were determined using the Axios
advanced wavelength dispersive XRF spectrometer (WD-
XRF; PANalytical) at the Laboratory of Soil Structure and
Mineralogy, Institute of Geology and Geophysics, Chinese
academy of sciences (CSA). We conducted a calibration
using 48 certified reference materials from China (26 soil
samples (GSS 1–26), 4 stream sediment samples (GSD 9–11,
20), and 18 rock samples (GSR 1–18)). The analysis un-
certainties were ±3% for all the elements.
3.4 TOC and C/N analysis
A total of 512 subsamples were collected from the same core
Sci China Earth Sci
depths as the traditional XRF samples for measurements of
total organic carbon (TOC), total nitrogen (TN), and organic
carbon to total nitrogen (C/N) ratios of sedimentary organic
matter. To remove inorganic carbonate, powdered samples
−1
were treated with 1 mol L CH3COOH for >10 h (Jackson,
1956) and then rinsed with deionised water and dried in an
oven at 40°C. The samples were then ground to 200 mesh
powder and homogenised. Powdered samples of 160–200 mg
(±0.01 mg) were weighed and placed in tin cups. The wrapped
samples were then folded and crimped to remove the air. TOC
and TN were measured on an elemental analyser (Vario
MACRO cube) at the Physicochemical Analysis Center, In-
stitute of Geographic Sciences and Natural Resources Re-
search, CAS. The C, N, and C/N ratios were calibrated using a
phenylalanine standard and expressed as a mass percentage.
The analytical precision was <0.1%.
4. Results
4.1 Rb/Sr ratios based on XRF core scanning and PCA
We produced a continuous high-resolution Rb/Sr record for
core ZB13-C1 (Figure 3a) in conjunction with records of
XRF scanned elements. Rb and Sr mainly displayed reversed
trends with high fluctuations throughout the core. Several
extreme Rb and Sr values occurred in organic matter layers
 Yang H, et al. Sci China Earth Sci 5

Figure 3 The XRF core-scanning results of core ZB13-C1 from the Zoige Basin on the eastern Tibetan Plateau. (a) The downcore variability of Rb, Sr, and
Rb/Sr ratios. The average Rb/Sr value of 0.38 is indicated by the dashed line, and the trend was filtered using a 20-point moving average (purple line). The Rb
and Sr curves were processed using a denary logarithm. (b) Correlation between Rb/Sr ratios and Sr and Rb.

(Figure 2), reflecting the dilution effect from organic matter.

We therefore used the Rb/Sr ratio to minimise this dilution
effect. As illustrated in Figure 3b, the XRFCS Rb/Sr ratios
were highly correlated with Sr (coefficient of determination
2 2
R =0.73) and weakly correlated with Rb (R =0.50). The Rb/
Sr ratios are therefore predominantly controlled by Sr ac-
tivity during weathering within the lake catchment.
For the PCA of Si, Al, Ti, K, Rb, Zr, Fe, Ca, and Sr, the
first two principal components (PC) extracted from the factor
load matrix accounted for 64.1% of the total variance (Figure
4). The first principal component (PC1) accounted for 39.6%
of the total variance and therefore predominantly contributed
toward the variability in the XRF elemental dataset. PC1 had
a strong positive loading from diagenetic elements (Si, Al,
Zr, K, Ti, Rb, and Fe) and a strong negative loading from
carbonate-associated elements (Sr and Ca) (Figure 4). Si, Al, Figure 4 The XRF elemental projections over the bi-plot of the first two
K, Ti, Rb, and Fe are diagenetic elements that represent the principal components (PC1 and PC2).
6 Yang H, et al.
siliciclastic fraction, while Sr and Ca likely originated from
authigenic carbonate (Wang et al., 1995a; Chen et al., 1999).
Therefore, we interpret PC1 to represent the relative change
of terrigenous material and authigenic material in the lake
sediment.
4.2 Traditional XRF results
The CIA index, carbonate-free Rb/Sr ratio, measured weight
percentage of Rb, carbonate-free Sr, and several oxides for
the calculation of CIA are displayed in Figure 5. Al2O3
concentrations ranged from 6 wt.% to 20 wt.%, and K2O
concentrations ranged from 1 wt.% to 4 wt.%. The Al2O3 and
K2O downcore trends showed good consistency (Figure 5)
* *
but significantly differed to that of Na2O and CaO . CaO
concentrations (mean value of 0.96 wt.%) were lower than
Figure 5 The traditional XRF results of core ZB13-C1 from the Zoige Basin on the eastern Tibetan Plateau. CaO represents the weight percentage of CaO in
*
silicate minerals. The horizontal dashed lines for Rb/Sr, CIA, Na2O, and CaO denote their average values of 1.46, 62.69, 1.97 wt.%, and 0.96 wt.%, respectively.
Sci China Earth Sci
that of Na2O (mean value of 1.97 wt.%) inferring almost
complete carbonate removal. Furthermore, the CIA index
ranged from 53 to 75 (average value of 62.69), while the
carbonate-free Rb/Sr ratios ranged from 0.5 to 3 (average
value of 1.46).
4.3 TN, TOC, and C/N
C/N values ranged from 1.92 to 24.26, with an average value
of 7.69 (Figure 6). The high TOC and TN values were po-
sitively correlated with the occurrence of organic matter
layers (Figure 2). Moreover, TOC and TN contents exhibited
a good correlation with C/N based on their corresponding
peaks. TOC significantly positively correlated with C/N ra-
2
tios (R =0.87), whereas TN was less correlated with C/N
2
(R =0.68); this suggests that C/N variability was pre-
*
 Yang H, et al. Sci China Earth Sci 7

Figure 6 The TOC, TN, and C/N results of core ZB13-C1 from the Zoige Basin on the eastern Tibetan Plateau. (a) Downcore trends in TOC, TN, and C/N
(dashed line is the average C/N value of 7.69); (b) correlation between C/N and TOC content; (c) correlation between C/N and TN content.

dominantly controlled by changes in TOC content.
5. Discussion
5.1 Comparison of XRFCS Rb/Sr with CIA
The Rb/Sr ratios of lake sediments have been widely used to
measure the chemical weathering intensity in lake catch-
ments (Jin and Zhang, 2002). Rb often appears in the form of
isomorphism in K-rich minerals, such as potassium feldspar
and mica, and is released during supergene weathering pro-
cesses. However, the released Rb tends to remain in the
source area, as it is easily re-absorbed by K-rich clays. As a
result, only a small portion of Rb is leached and transported
to the lake via surface runoff (Pang et al., 2001). In contrast,
Sr is transported via surface runoff in the form of free
strontium during chemical weathering; this increases the
strontium input to lake sediments through physical adsorp-
tion (onto organic matter) and/or chemical precipitation
(carbonate) (Wedepohl, 1978). Therefore, the Rb/Sr varia-
bility in lake sediments can indicate past chemical weath-
ering intensity in lake catchments.
CIA is also considered a suitable proxy for chemical
weathering in lake catchments. CIA was initially used to
assess the in situ weathering degree of feldspar minerals,
consisting of aluminum silicate (Nesbitt and Young, 1982).
The removal of calcium, sodium, and potassium from feld-
spars during chemical weathering increases the proportion of
alumina to alkalis in weathering residues. However, free
calcium, sodium, and potassium are transported to lake se-
8 Yang H, et al. Sci China Earth Sci

diments via surface runoff during intensive chemical
weathering, which lowers the CIA values (An et al., 2011).
We compared the downcore sedimentary variations of
these two chemical weathering indicators (XRFCS Rb/Sr ratio
and CIA index) in the Zoige Basin. Their trends were gen-
erally comparable throughout the core (Figure 7a); however,
their modest positive correlation (r=0.45) may be due to their
deviation in some sedimentary intervals (Figure 7b). The
entire sedimentary sequence of core ZB13-C1 was therefore
divided into four units based on lithology: unit I is composed
of 62% clay (104–78.62 m), unit II is composed of 62% silty
clay (78.62–35.51 m), unit III is composed of 66% silt
(35.51–25 m), and unit IV is composed of 45% fine sand
(25–0.3 m) (Figure 7a). A scatter plot of Rb/Sr and CIA in
each unit showed decreasing correlation coefficients from
unit 4 to unit 1 (Figure 7c). This suggests that Rb/Sr and CIA
in clay components are more reliable proxies of chemical
weathering intensity.
5.2 Indication of XRFCS Rb/Sr ratios and CIA
The chemical composition of lake sediments is often in-
fluenced by multiple factors, such as the composition of the
source provenance, sediment transport, depositional en-
vironment, and chemical processes during weathering,
transport, and burial (Bjørlykke, 2010). We therefore dis-
cussed the indication of Rb/Sr and CIA in detail to elim-
inate the influence of other factors on Rb/Sr and CIA
variability.
The Zoige paleolake was considered a closed system
during the period of paleolake deposition (Sheng, 2007). The
lake sediment deposits were predominantly terrigenous and
sourced from eroded rocks or weathered soils in the catch-
ment via surface runoff and/or aeolian transport (Hakanson
and Jansson, 1983). The magmatic activity in the Zoige
block was relatively weak, and its caprock consists mainly of
Triassic light metamorphic sandstone, shale, and carbonac-

Figure 7 Comparisons of XRFCS Rb/Sr with CIA of core ZB13-C1. (a) Downcore comparison between Rb/Sr and CIA for core ZB13-C1. The horizontal
dashed lines for CIA and Rb/Sr denote their average values of 62.69 and 0.38, respectively. The vertical dotted lines connecting Rb/Sr and CIA mark the
sedimentary intervals where they exhibit the same variation. (b) Scatter plot of Rb/Sr and CIA for the entire sedimentary sequence. (c) Scatter plot of Rb/Sr
and CIA for the four sedimentary units.
 Yang H, et al. Sci China Earth Sci 9

prock has a single lithology and the sedimentary basin has a

Figure 8 Scatter plot of TiO2/Nb and Nb/Al2O3 for core ZB13-C1.
eous slate (Xu, 1988; Bureau of Geology and Mineral Re-
sources of Sichuan Province, 1991). The sedimentary ca-
small provenance range; the influence of a changing source
on the chemical composition of the lake sediment is therefore
negligible. Moreover, according to the graphical analysis of
element pairs introduced by Fralick and Kronberg (1997),
the scatter plot of chemically immobile elemental ratios in
sediments reflects the weighted average composition of the
source rock. The elemental ratios would scatter on the plot if
the source rock composition was variable and the sediments
were not well mixed before deposition. Al, Ti, and Nb are
considered essentially immobile during weathering pro-
cesses (MacLean and Hoy, 1991; Fralick and Kronberg,
1997). Except for five datapoints derived from organic-rich
layers, Al2O3-TiO2-Nb ratios for core ZB13-C1 showed a
linear trend on the scatter plot rather than a dispersion
(Figure 8), indicating uniform source rock composition. We
therefore assume that the composition of the source rock
cannot explain the variations in Rb/Sr and CIA.
With regard to lake sediment transport processes, the se-
diment geochemical variability predominantly reflects the

Figure 9 Downcore comparisons of CIA, XRFCS Rb/Sr, PC1 score, carbonate content (Ren, 2020), and mean grain size (Ren, 2020) of core ZB13-C1 from
the Zoige Basin. The horizontal dashed lines for CIA and Rb/Sr denote their average values of 62.69 and 0.38, respectively. The pink horizontal lines for
mean grain size represent the average values of the different sedimentary sequences. The blue dashed lines mark the peaks in grain size related to organic
matter and carbonate layers rather than silicates.
10 Yang H, et al.
grain-size changes via hydraulic or aerodynamic sorting. For
example, a decrease in Ti/K and an increase in Fe/Ti indicate
a reduction in grain size driven by a decrease in energy for
sediment transport (Marshall et al., 2011). The simulta-
neously changes in Ti/Al, Rb/Al, and Zr/Al in the sedi-
mentary sequence of Lake Stymphalia (NE-Peloponnese)
were indicative of torrential riverine input and were asso-
ciated with clastic mineral and/or clay mineral assemblages
(Heymann et al., 2013). Moreover, the immobile elements,
such as Ti, Zr and Al, are the most susceptible to transport
and are predominantly unaffected by weathering and redox
processes during transport. Easily dissolved and weathered
elements, such as Ca, Na, K, and Sr, are more suitable in-
dicators of chemical weathering intensity than conservative
geochemical elements; the Rb/Sr and CIA proxies are based
on this rationale (Dasch, 1969; Nesbitt and Young, 1982).
Furthermore, the sedimentation rate of core ZB13-C1 was
relatively stable throughout the entire sequence (Ren, 2020).
The influence of high detrital deposition on Rb/Sr and CIA
was therefore negligible.
The mean grain size (Ren, 2020) of core ZB13-C1 was
used as a proxy for transport energy (mainly waterflow)
(Francke et al., 2013; Dietze et al., 2014), and the PC1 score
—which is indicative of the relative change of terrigenous
material and authigenic material—was compared with Rb/Sr
and CIA. We identified no obvious change in mean grain size
in sedimentary units I and II when excluding organic matter
and carbonate layers (Figure 9); this suggests negligible in-
fluence of changing transport mechanisms on the sediment
chemical composition. Furthermore, the carbonate-dominant
intervals corresponded to low Rb/Sr and CIA values. Ac-
cording to the carbonate record of core RH located ~16 km
west of core ZB13-C1, the carbonate preserved in Zoige
paleolake sediment is dominated by authigenic minerals
(Wang et al., 1995a; Chen et al., 1999). The Rb/Sr variability
was predominantly dependent on Sr activity (Figure 3b).
During intensified chemical weathering, Sr is heavily lea-
ched from its source area in the lake catchment and is sub-
2+
sequently transported to the lake as Sr ions in surface
2+
runoff. The dissolved Sr would be preferentially in-
corporated into authigenic carbonate (chemical precipita-
tion) and/or attracted to organic matter in the lake (Chang et
al., 2013). In contrast, the Rb/Sr ratios and CIA exhibit high
values in sedimentary intervals of low carbonate and high
terrigenous material, indicating a weakened leaching of Sr in
the lake catchment. Therefore, the Rb/Sr ratio and CIA in the
fine-grained clay of units I and II can reliably reflect past
chemical weathering intensity.
The increase in mean grain size in the early depositional
period of unit III (Figure 9) indicates enhanced transport
energy from intensified rainfall. High rainfall during this
interval would enhance chemical weathering and lower the
values of Rb/Sr and CIA, despite the lower carbonate content
Sci China Earth Sci
to that of 28–25 m. Therefore, we conclude that Rb/Sr and
CIA recorded in unit III are sensitive to changes in chemical
weathering intensity.
Unit IV consists of 45% fine sand and is dominated by
terrigenous material (Figure 9). The mean grain size in this
unit was highly variable, and we observed a number of low
Rb/Sr and CIA values (especially Rb/Sr). The Zoige paleo-
lake was pirated by the Yellow River at 38–35 ka BP based
on the sedimentological increase in the sand fraction (Wang
et al., 1995b). After this, the lake deposits were replaced by
fluvial deposits. The enhanced and highly variable mean
grain size may therefore indicate the fluvial facies in core
ZB13-C1 and represent a change in the depositional en-
vironment; thus, the Rb/Sr and CIA in unit 1 cannot solely
reflect changes in chemical weathering intensity.
5.3 Correlation of XRFCS Rb/Sr ratios with paleocli-
mate proxies in the Zoige Basin
To further verify whether XRFCS Rb/Sr ratios are adequate
indicators of both chemical weathering and the Asian sum-
mer monsoon intensity, we compared the XRFCS Rb/Sr ratio
and CIA with TOC content, C/N ratios, and other previously
measured paleoclimate indicators from core ZB13-C1 (Ren,
2020) (Figure 10). The peak values of TOC content, C/N
ratios, AP content, and carbonate content correlated well
with low Rb/Sr and CIA values (Figure 10).
The C/N ratio has been widely used to distinguish between
the different sources of organic matter in lake sediments (Xu
et al., 2017; Lan et al., 2019). The C/N ratios of aquatic
plants are typically lower than 7, while those of terrestrial
plants and their humic substances are >20 (Aitkenhead and
McDowell, 2000; Vane et al., 2013a, 2013b; Khan et al.,
2015). C/N ratios between 7 and 20 usually represent a
mixed source of organic matter from both terrigenous input
and lake endogenous accumulation (Meyers, 1994). TOC
typically reflects the primary productivity in lakes (Wu et al.,
2006; Liu et al., 2018). In our study, extremely high TOC
values (>20%) occurred in conjunction with high values of
C/N (>7) (Figure 10), indicating increased terrigenous or-
ganic material in lake sediment. The high TOC values may
be due to increased transport of terrigenous organic material
and nutrients in response to enhanced rainfall and surface
runoff.
High AP and carbonate contents corresponded to low Rb/
Sr and CIA values (Figure 10). AP variability in the Zoige
Basin is related to changes in summer temperature (Shen C
M et al., 2006). An increase in the proportion of AP indicates
forest expansion in the lake catchment under favourable
hydrothermal conditions. Furthermore, high-carbonate in-
tervals correspond to high lake levels in the Zoige Basin
(Zhao et al., 2020). This optimum hydrothermal condition in
the Zoige Basin (indicated by peaks in AP, carbonate, TOC,
 Yang H, et al. Sci China Earth Sci 11

Figure 10 Downcore comparisons of paleoclimate conditions based on multiple proxies from core ZB13-C1 from the Zoige Basin, including TOC, C/N,
AP (Ren, 2020), CIA, XRFCS Rb/Sr, and carbonate content (Ren, 2020). The XRFCS Rb/Sr data were filtered using a 20-point moving average (in purple line).
The dashed lines for CIA and the XRFCS Rb/Sr denote their average values of 62.69 and 0.38, respectively. Vertical grey bars represent warm and humid
climatic periods.

and C/N; Figure 10) likely accelerated the chemical weath-
ering rate and lowered the Rb/Sr ratio and CIA values in the
lake sediment.
The Zoige Basin is located in the monsoonal region of the
TP (Figure 1) and is therefore highly sensitive to the Asian
monsoon (Ye and Gao, 1979; Ding, 1992). The Zoige Basin
consists of the most extensive distribution of high-altitude
peat bogs. Studies have shown that the warm and moist air
transported by the Indian summer monsoon played a domi-
nant role in forming the widespread peat bogs of the Zoige
Basin (Wang et al., 2004). Previous studies have explored
several monsoon proxies derived from peat sections in the
Zoige Basin, such as ash content (indicator of winter mon-
13
soon), grayscale, humification degree, and δ C of Carex
mulieensis cellulose (indicator of summer monsoon) (Zhou
et al., 2001; Hong et al., 2003; Yu et al., 2006). The corre-
lations between these indices and the Asian monsoon are
based on their links with temperature and precipitation.
Temperature and precipitation are also the dominant factors
controlling the direction and intensity of chemical weath-
ering (Zhang, 1997). The chemical weathering of carbonate,
plagioclase, mafic, and sulfide minerals were enhanced
12 Yang H, et al.
during the strong monsoon interval, resulting in the increased
lacustrine transport of more labile oxides and dissolved ions
2+ 2+ 2+ 2+ + +
(e.g., Ca , Sr , Mg , Fe , Na , K , etc.); this in turn re-
duced the Rb/Sr and CIA values of the lake sediments (An et
al., 2011). Based on the comparisons of Rb/Sr and CIA with
other paleoclimatic indicators (TOC, AP, carbonate content,
and C/N ratios), we confirm the validity of XRFCS Rb/Sr as
an accurate proxy for chemical weathering and Asian sum-
mer monsoon intensities.
5.4 Grain-size influence on XRFCS Rb/Sr ratios
Grain size is an important variable that influences the in-
terpretation of chemical weathering indices (Xiong et al.,
2010). To investigate the relationships between CIA and Rb/
Sr ratio with grain size, we conducted a correlation analysis
on CIA index; XRFT Al2O3, K2O, Na2O, CaO, Rb/Sr, Rb, and
Sr; XRFCS Rb/Sr, Rb, and Sr; and grain size (Ren, 2020)
(Figure 11). Organic matter and carbonate layers do not re-
flect the silicate grain-size variability considering their sig-
nificantly higher mean grain size values (Figure 9). We
therefore excluded the grain-size data of organic matter and
carbonate-rich intervals and their corresponding geochem-
ical data prior to the correlation analysis. Furthermore, the
top ca. 25-m sequence of core ZB13-C1 is dominated by
coarse-grained sediments, while the deeper sequence is
mainly composed of finer silt and clay (Figure 9). We
therefore conducted separate correlation analyses on the two
sedimentary sequences (104–25 and 25–0.3 m).
For the 104–25 m sedimentary sequence, we identified
Pearson correlation coefficients of −0.64 between CIA and
mean grain size and −0.42 between XRFT Rb/Sr and mean
grain size (Figure 11). Moreover, the XRFCS Rb/Sr was
weakly negatively correlated with mean grain size (r=−0.33).
The weak correlations between the XRFT and XRFCS Rb/Sr
ratios with mean grain size is due to the association of Rb
with the clay fraction (r=0.27 and 0.33), as Rb strongly sorbs
onto clay minerals. Moreover, we observed a correlation
coefficient of −0.23 between the XRFT Sr and the clay
fraction, while the XRFCS Sr showed no correlation with the
clay, silt, or sand fractions. Sr is relatively insensitive to
grain-size variations, as it is preferentially incorporated into
carbonate minerals (such as calcite and aragonite) in the lake
sediments of core ZB13-C1 (Croudace and Rothwell, 2015).
As the XRFCS Rb/Sr ratios are predominantly dependent on
Sr activity during weathering, the XRFCS Rb/Sr ratios would
rarely be influenced by grain size when used as proxy for
chemical weathering intensity.
For the 25–0.3 m sedimentary sequence, we identified a
Pearson correlation coefficient of −0.23 between CIA and
mean grain size and 0.38 between XRFT Rb/Sr and mean
grain size (Figure 11). We also observed no correlation be-
tween the XRFCS Rb/Sr ratios and mean grain size. The weak
Sci China Earth Sci
correlation between CIA and mean grain size is due to the
association between grain size and chemical composition. As
illustrated in Figure 11, Al2O3 and K2O are highly correlated
with the clay fraction (grain size <4 μm), with correlation
coefficients of 0.7 and 0.62, respectively. The correlation
between grain size and the geochemical composition of se-
diments is related to particular elements with varying mi-
neral characteristics, including different densities, grain
sizes, and shapes (Volborth, 1969). The most abundant ma-
terials in the clay-sized fraction of lake sediments are illite,
kaolinite, and chlorite, which can absorb many elements,
including Cs, K, and Rb (Cohen, 2003; Croudace and
Rothwell, 2015). Under supergene weathering, clay minerals
are formed by the chemical reaction between aluminium
silicate and pore fluid (Chamley, 1989). Clays are therefore
rich in Al and K, as kaolinite and illite are mainly composed
of Al2O3 and K2O, respectively (Wehausen and Brumsack,
2000; Hebbeln et al., 2006). We observed a high correlation
between CIA and the clay fraction (r=0.68) (Figure 11), as
CIA is calculated from Al2O3, K2O, Na2O, and CaO. Simi-
larly, the positive correlation between XRFT Rb/Sr and mean
grain size is due to the association between Sr content and the
silt fraction (r=0.51). As the carbonate was removed from the
samples, the XRFT Sr data represent the preserved Sr in non-
carbonate minerals.
Grain size can influence the XRF core-scanned data and
subsequently impact the XRFCS Rb/Sr ratios. The sediment
physical properties—particularly grain size—are known to
influence in situ XRF scanning results (Croudace et al.,
2006). Analysis errors may arise from irregular core surfaces
caused by varying grain sizes, which can result in the in-
homogeneous absorption of incident X-rays (Luo et al.,
2008). To evaluate the influence of grain size on the XRFCS
Rb/Sr ratios, we applied a 10-m moving correlation analysis
on the XRFT Rb/Sr and Rb, the XRFCS Rb/Sr and Rb, and the
CIA index throughout the core. The correlation coefficients
between XRFT Rb/Sr and XRFCS Rb/Sr showed low and
negative values in the three sedimentary sequences (25–0.3,
56–50.03, and 86.95–83.95 m) (Figure 12), inferring the low
accuracy of scanned Rb/Sr ratios in all sequences. As the
XRFT Rb/Sr was determined on carbonate-free samples, the
measured Sr of discrete samples and the scanned Sr of the
bulk core are not directly comparable. We therefore con-
ducted another moving correlation analysis on XRFT Rb and
XRFCS Rb, as the carbonate removal in samples would not
affect the Rb content in the lake sediments. In agreement
with the Rb/Sr moving correlation, the correlation coefficient
between Rb measurements from the two XRF methods were
low and negative in all three sequences (Figure 12). This
infers the poor accuracy of the scanned results in all three
sedimentary sequences, which explains the low and negative
correlation between CIA and the XRFCS Rb/Sr at depths of
25–0.3 and 56–47 m. However, we did not observe a reverse
 Yang H, et al.
Figure 11 Pearson correlation coefficients (r) between XRFCS data, XRFT data, and grain size data for sedimentary sequences 104–25 and 25–0.3 m. XRFCS
data includes XRFCS Rb/Sr, XRFCS Rb, and XRFCS Sr. XRFT data includes CIA, Al2O3, K2O, Na2O, CaO, XRFT Rb/Sr, XRFT Rb, and XRFT Sr. Grain size
data includes mean grain size (µm), clay fraction content (grain size <4 μm), silt fraction content (grain size of 4–63 μm), and sand fraction content (grain size
>63 μm) (Ren, 2020).
relationship between CIA and the XRFCS Rb/Sr ratios in the
83.95–86.95 m sequence, despite the negative correlation
coefficient between the two Rb/Sr ratios. It is notable that a
ca. 2 m thick organic matter layer and a sedimentary gap of
ca. 0.8 m are included in the 86.95–83.95 m sequence; this
means nearly half of the geochemical data has been excluded
prior to the moving correlation analysis. We therefore as-
sume accurate XRF core-scanned results at 86.95–83.95 m
depth considering the organic matter layer and sedimentary
gap, which likely influenced the correlation between the
XRFCS Rb/Sr ratios and XRFT Rb/Sr ratios.
The grain size in the 25–0.3 m sequence (lithological unit
1) is highly variable and predominantly coarse (Figure 12).
The XRF core-scanned results are therefore likely to be in-
fluenced by grain size in this sequence, and the XRFCS Rb/Sr
ratios may inaccurately reflect the chemical weathering in-
tensity of the lake catchment. However, the fine-grained
section characterised by moderate grain-size variability is
likely to have higher precision. The exception is sequence
56–47 m, in which the XRFCS Rb/Sr ratios showed low ac-
curacy based on the moving correlation analysis between
CIA, XRFCS Rb/Sr, and XRFT Rb/Sr. Consequently, the
XRFCS Rb/Sr ratios at 56–47 m depth inaccurately reflect the
chemical weathering intensity in the lake catchment.
For carefully treated and highly constrained sediment
cores, XRF-scanned element variability will predominantly
reflect changes in chemical composition rather than grain
size or depositional processes (Hunt et al., 2015). Only ele-
ments that are highly sensitive to grain-size changes—such
Sci China Earth Sci 13
as Zr, Ti, Fe, and K—can be assessed (as their normalised
individual datasets or as ratios) to identify grain-size changes
downcore (Dypvik and Harris, 2001; Wennrich et al., 2014;
Liu et al., 2019). Nevertheless, our study highlights the need
for mutual verification among multiple indicators in other
study regions to accurately interpret the paleoclimatic
variability.
6. Conclusions
We conducted a multi-proxy analysis of paleolake sediments
from the Zoige Basin to assess the application of XRFCS Rb/
Sr ratios as a proxy for chemical weathering and Asian
summer monsoon intensities. The observed correlations be-
tween Rb/Sr, CIA, and other paleoclimatic indicators (TOC,
C/N ratio, AP, and carbonate content) highlight the potential
of XRFCS Rb/Sr ratios to reflect both the intensity of che-
mical weathering and the strength of the Asian summer
monsoon in the Zoige paleolake catchment. Based on the
correlation analysis, grain size in the highly fluctuating
coarse-grained sequence at 25–0.3 m was found to influence
the XRFcs Rb/Sr data. In contrast, the precision of XRFcs Rb/
Sr ratios increased in the moderately fluctuating fine-grained
sequence at 104–25 m, with the exception of sequence
56–47 m, in where the XRFcs Rb/Sr ratios were considered in
poor accuracy. Therefore, the XRFCS Rb/Sr ratios of se-
quences 25–0.3 and 56–47 m are unlikely to adequately re-
flect chemical weathering intensity and should be excluded
14 Yang H, et al. Sci China Earth Sci

Figure 12 The 10-m moving correlation analysis between CIA and XRFCS Rb/Sr, XRFT Rb/Sr and XRFCS Rb/Sr, and XRFT Rb and XRFCS Rb. The
rectangles plotted on the correlation coefficient profiles denote the sedimentary sequences with low and negative correlation coefficients. The pink horizontal
lines for mean grain size (Ren, 2020) represent the average values of the four lithological units. The mean grain size data of organic matter and carbonate
layers were excluded.

for paleoclimatic reconstructions. Our study highlights the
need for mutual verification among multiple indicators be-
fore accurately applying Rb/Sr as a proxy for chemical
weathering intensity in other similar study areas.
Acknowledgements We acknowledge the two anonymous reviewers
for their constructive comments and suggestions. We thank Bin HU, Dandan
SUN, Xinhang WANG, Huiyang ZHOU, Chenhui HU, Liwen PENG, and
Weiling ZU for their assistance in the laboratory. This work was supported
by the Strategic Priority Research Program of Chinese Academy of Sciences
(Grant No. XDA20070101), the National Natural Science Foundation of
China (Grant Nos. 41690113 & 41888101), and the National Key Research
and Development Program of China (Grant No. 2016YFA0600501).
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(Responsible editor: Haibin WU)